Electronic structure engineering of Ru-doped Ni-based-LDH toward high-performance seawater electrolysis

Direct seawater electrolysis offers a sustainable pathway for large-scale hydrogen production but is fundamentally limited by chloride-induced corrosion, parasitic chlorine chemistry, and rapid catalyst degradation at industrial current densities. Here, we report a Ru-doped Ni-based-layered double hydroxide integrated with a pyrolyzed wood-derived carbon scaffold (NiRu-LDH@pWD) that addresses these issues through synergistic electronic structure and electrode architecture engineering. Ru doping reconfigures the local electronic environment of Ni, strengthens Ni–O coordination, downshifts the d -band center, and suppresses Cl∗ adsorption, thereby enhancing catalytic selectivity and stability in chloride-rich electrolytes. Concurrently, Ru doping induced lattice modulation promotes preferential exposure of catalytically active (012) edge planes. The hierarchically porous pWD carbon scaffold enables rapid charge transport, efficient ion diffusion, and superaerophobic gas release, sustaining high-rate operation. As a result, the NiRu-LDH@pWD electrode delivers low overpotentials for HER (74.7 mV in 1 M KOH and 101.1 mV in seawater) and OER (240 mV in 1 M KOH and 260 mV in seawater) at 10 A cm −2 , and exhibits >1000 h operational durability at 1 A cm −2 in seawater. An anion exchange membrane water electrolyzer assembled with NiRu-LDH@pWD achieves a low cell voltage of 2.01 V at 1 A cm −2 with negligible performance decay, meanwhile techno-economic analysis estimates a competitive hydrogen production cost of ∼US$0.35 kg −1 by ASPEN calculation. This work establishes an integrated strategy that couples atomic-scale electronic regulation with macroscopic electrode design to enable selective, durable, and economically viable seawater electrolysis.